We obtained excellent Laue diffraction photographs from crystals of trimethylamine dehydrogenase (TMADH). We collected Laue data sets from native and substrate bound crystals at several different pH values. Using the substrate, dimethylethylamine (DEMA), we were able to obtain data at pH 7.5 without damaging the crystal. The spin-interacting state is formed under these conditions based on microspectrophotometric measurements. The data sets were incomplete (only 30%) due to a number of factors, thus interpretable electron density maps could not be produced.